ADVANCED SULFUR CONTROL CONCEPTS FOR HOT-GAS DESULFURIZATION TECHNOLOGY

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This research project examined the feasibility of a second generation high-temperature coal gas desulfurization process in which elemental sulfur is produced directly during the sorbent regeneration phase. Two concepts were evaluated experimentally. In the first, FeS was regenerated in a H2O-O2 mixture. Large fractions of the sulfur were liberated in elemental form when the H2O-O2 ratio was large. However, the mole percent of elemental sulfur in the product was always quite small (<<1%) and a process based on this concept was judged to be impractical because of the low temperature and high energy requirements associated with condensing the sulfur. The ... continued below

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ORTIZ, A. LOPEZ; HARRISON, D.P.; GROVES, F.R.; WHITE, J.D.; ZHANG, S.; HUANG, W.-N. et al. October 31, 1998.

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This research project examined the feasibility of a second generation high-temperature coal gas desulfurization process in which elemental sulfur is produced directly during the sorbent regeneration phase. Two concepts were evaluated experimentally. In the first, FeS was regenerated in a H2O-O2 mixture. Large fractions of the sulfur were liberated in elemental form when the H2O-O2 ratio was large. However, the mole percent of elemental sulfur in the product was always quite small (<<1%) and a process based on this concept was judged to be impractical because of the low temperature and high energy requirements associated with condensing the sulfur. The second concept involved desulfurization using CeO2 and regeneration of the sulfided sorbent, Ce2O2S, using SO2 to produce elemental sulfur directly. No significant side reactions were observed and the reaction was found to be quite rapid over the temperature range of 500°C to 700°C. Elemental sulfur concentrations (as S2) as large as 20 mol% were produced. Limitations associated with the cerium sorbent process are concentrated in the desulfurization phase. High temperature and highly reducing coal gas such as produced in the Shell gasification process are required if high sulfur removal efficiencies are to be achieved. For example, the equilibrium H2S concentration at 800°C from a Shell gas in contact with CeO2 is about 300 ppmv, well above the allowable IGCC specification. In this case, a two-stage desulfurization process using CeO2 for bulk H2S removal following by a zinc sorbent polishing step would be required. Under appropriate conditions, however, CeO2 can be reduced to non-stoichiometric CeOn (n<2) which has significantly greater affinity for H2S. Pre-breakthrough H2S concentrations in the range of 1 ppmv to 5 ppmv were measured in sulfidation tests using CeOn at 700°C in highly reducing gases, as measured by equilibrium O2 concentration, comparable to the Shell gas. Good sorbent durability was indicated in a twenty-five-cycle test. The sorbent was exposed for 58 consecutive days to temperatures between 600°C and 800°C and gas atmospheres from highly reducing to highly oxidizing without measurable loss of sulfur capacity or reactivity. In the process analysis phase of this study, a two-stage desulfurization process using cerium sorbent with SO2 regeneration followed by zinc sorbent with dilute O2 regeneration was compared to a single-stage process using zinc sorbent and O2 regeneration with SO2 in the regeneration product gas converted to elemental sulfur using the direct sulfur recovery process (DSRP). Material and energy balances were calculated using the process simulation package PRO/II. Major process equipment was sized and a preliminary economic analysis completed. Sorbent replacement rate, which is determined by the multicycle sorbent durability, was found to be the most significant factor in both processes. For large replacement rates corresponding to average sorbent lifetimes of 250 cycles or less, the single-stage zinc sorbent process with DSRP was estimated to be less costly. However, the cost of the two-stage cerium sorbent process was more sensitive to sorbent replacement rate, and, as the required replacement rate decreased, the economics of the two-stage process improved. For small sorbent replacement rates corresponding to average sorbent lifetimes of 1000 cycles or more, the two-stage cerium process was estimated to be less costly. In the relatively wide middle range of sorbent replacement rates, the relative economics of the two processes depends on other factors such as the unit cost of sorbents, oxygen, nitrogen, and the relative capital costs.

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  • Other: DE00007129
  • Report No.: DE-AC21-94MC30012--18
  • Grant Number: AC21-94MC30012
  • DOI: 10.2172/7129 | External Link
  • Office of Scientific & Technical Information Report Number: 7129
  • Archival Resource Key: ark:/67531/metadc709370

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  • October 31, 1998

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  • Sept. 12, 2015, 6:31 a.m.

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  • Dec. 8, 2016, 2:16 p.m.

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ORTIZ, A. LOPEZ; HARRISON, D.P.; GROVES, F.R.; WHITE, J.D.; ZHANG, S.; HUANG, W.-N. et al. ADVANCED SULFUR CONTROL CONCEPTS FOR HOT-GAS DESULFURIZATION TECHNOLOGY, report, October 31, 1998; Morgantown, West Virginia. (digital.library.unt.edu/ark:/67531/metadc709370/: accessed June 20, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.